Due to continuously stricter regulations regarding emissions from power generation processes, further development of existing gas turbine combustors is essential. A promising alternative to conventional flame combustion in gas turbines is catalytic combustion, which can result in ultralow emission levels of NOx, CO and unburned hydrocarbons. The work presented in this thesis concerns the development of methane oxidation catalysts for gas turbine combustors. The application of catalytic combustion to different combustor concepts is addressed in particular. The first part of the thesis (Paper I) reports on catalyst development for fuel-lean methane combustion. Supported Pd-based catalysts were investigated at atmospheric pressure. The effect on catalytic activity of diluting the reaction mixture with water and/or carbon dioxide was studied in order to simulate a combustion process with exhaust gas recirculation. The catalytic activity was found to decrease significantly in the presence of water and CO2. However, modifying the catalyst by changing support material can have a considerable impact on the performance. In the second part of this thesis (Papers II-IV), the development of rhodium catalysts for fuel-rich methane combustion is addressed. The effect of catalyst composition, oxygen-to-fuel ratio and catalyst pre-treatment on the methane conversion and the product gas composition was studied. An experimental investigation at elevated pressures of partial oxidation of methane/oxygen mixtures in exhaust gas-rich environments was also conducted. The most suitable catalyst identified for fuel-rich catalytic combustion of methane, i.e. Rh/Ce-ZrO2, showed benefits such as low light-off temperature, high activity and enhanced hydrogen selectivity. In the final part of the thesis (Paper V), a numerical investigation of fuel-rich catalytic combustion is presented. Measurements and predictions were compared for partial oxidation of methane in exhaust gas diluted mixtures at elevated pressures. The numerical model was validated for several Rh-based catalysts. The key parameter controlling the catalytic performance was found to be the noble metal dispersion. / QC 20110125

<p>Due to continuously stricter regulations regarding emissions from power generation processes, further development of existing gas turbine combustors is essential. A promising alternative to conventional flame combustion in gas turbines is catalytic combustion, which can result in ultralow emission levels of NO_x, CO and unburned hydrocarbons. The work presented in this thesis concerns the development of methane oxidation catalysts for gas turbine combustors. The application of catalytic combustion to different combustor concepts is addressed in particular.</p><p>The first part of the thesis (Paper I) reports on catalyst development for fuel-lean methane combustion. Supported Pd-based catalysts were investigated at atmospheric pressure. The effect on catalytic activity of diluting the reaction mixture with water and/or carbon dioxide was studied in order to simulate a combustion process with exhaust gas recirculation. The catalytic activity was found to decrease significantly in the presence of water and CO₂. However, modifying the catalyst by changing support material can have a considerable impact on the performance.</p><p>In the second part of this thesis (Papers II-IV), the development of rhodium catalysts for fuel-rich methane combustion is addressed. The effect of catalyst composition, oxygen-to-fuel ratio and catalyst pre-treatment on the methane conversion and the product gas composition was studied. An experimental investigation at elevated pressures of partial oxidation of methane/oxygen mixtures in exhaust gas-rich environments was also conducted. The most suitable catalyst identified for fuel-rich catalytic combustion of methane, i.e. Rh/Ce-ZrO₂, showed benefits such as low light-off temperature, high activity and enhanced hydrogen selectivity.</p><p>In the final part of the thesis (Paper V), a numerical investigation of fuel-rich catalytic combustion is presented. Measurements and predictions were compared for partial oxidation of methane in exhaust gas diluted mixtures at elevated pressures. The numerical model was validated for several Rh-based catalysts. The key parameter controlling the catalytic performance was found to be the noble metal dispersion.</p>